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An aza‐crown ether, modified phosphoramidite ligand, has been designed and synthesized. The ON/OFF reversible switch of catalytic activity for its rhodium catalyst was thoroughly investigated in the asymmetric hydrogenation of dehydroamino acid esters modulated by host–guest interactions. In the OFF state, the catalyst is almost inactive (less than 1 % conversion) because of the formation of an intermolecular...
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